EP1561509B1 - Catalyseur pour la purification des gaz d'échappement - Google Patents

Catalyseur pour la purification des gaz d'échappement Download PDF

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EP1561509B1
EP1561509B1 EP04293173A EP04293173A EP1561509B1 EP 1561509 B1 EP1561509 B1 EP 1561509B1 EP 04293173 A EP04293173 A EP 04293173A EP 04293173 A EP04293173 A EP 04293173A EP 1561509 B1 EP1561509 B1 EP 1561509B1
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honeycomb
shaped support
upstream
exhaust
gas purifying
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German (de)
English (en)
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EP1561509A1 (fr
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Junya c/o Cataler Corporation Shirahata
Kohei c/o Cataler Corporation Tomiyasu
Kazunori c/o Cataler Corporation Ito
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Cataler Corp
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Cataler Corp
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D46/00—Filters or filtering processes specially modified for separating dispersed particles from gases or vapours
    • B01D46/24—Particle separators, e.g. dust precipitators, using rigid hollow filter bodies
    • B01D46/2403—Particle separators, e.g. dust precipitators, using rigid hollow filter bodies characterised by the physical shape or structure of the filtering element
    • B01D46/2418—Honeycomb filters
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D46/00—Filters or filtering processes specially modified for separating dispersed particles from gases or vapours
    • B01D46/24—Particle separators, e.g. dust precipitators, using rigid hollow filter bodies
    • B01D46/2403—Particle separators, e.g. dust precipitators, using rigid hollow filter bodies characterised by the physical shape or structure of the filtering element
    • B01D46/2418—Honeycomb filters
    • B01D46/2451—Honeycomb filters characterized by the geometrical structure, shape, pattern or configuration or parameters related to the geometry of the structure
    • B01D46/2455—Honeycomb filters characterized by the geometrical structure, shape, pattern or configuration or parameters related to the geometry of the structure of the whole honeycomb or segments
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D46/00—Filters or filtering processes specially modified for separating dispersed particles from gases or vapours
    • B01D46/56—Filters or filtering processes specially modified for separating dispersed particles from gases or vapours with multiple filtering elements, characterised by their mutual disposition
    • B01D46/62—Filters or filtering processes specially modified for separating dispersed particles from gases or vapours with multiple filtering elements, characterised by their mutual disposition connected in series
    • B01D46/64—Filters or filtering processes specially modified for separating dispersed particles from gases or vapours with multiple filtering elements, characterised by their mutual disposition connected in series arranged concentrically or coaxially
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/92—Chemical or biological purification of waste gases of engine exhaust gases
    • B01D53/94—Chemical or biological purification of waste gases of engine exhaust gases by catalytic processes
    • B01D53/9445—Simultaneously removing carbon monoxide, hydrocarbons or nitrogen oxides making use of three-way catalysts [TWC] or four-way-catalysts [FWC]
    • B01D53/945—Simultaneously removing carbon monoxide, hydrocarbons or nitrogen oxides making use of three-way catalysts [TWC] or four-way-catalysts [FWC] characterised by a specific catalyst
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/92—Chemical or biological purification of waste gases of engine exhaust gases
    • B01D53/94—Chemical or biological purification of waste gases of engine exhaust gases by catalytic processes
    • B01D53/9445—Simultaneously removing carbon monoxide, hydrocarbons or nitrogen oxides making use of three-way catalysts [TWC] or four-way-catalysts [FWC]
    • B01D53/9454—Simultaneously removing carbon monoxide, hydrocarbons or nitrogen oxides making use of three-way catalysts [TWC] or four-way-catalysts [FWC] characterised by a specific device
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
    • B01J23/40—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals of the platinum group metals
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
    • B01J23/40—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals of the platinum group metals
    • B01J23/44—Palladium
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
    • B01J23/40—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals of the platinum group metals
    • B01J23/46—Ruthenium, rhodium, osmium or iridium
    • B01J23/464—Rhodium
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J35/00—Catalysts, in general, characterised by their form or physical properties
    • B01J35/19—Catalysts containing parts with different compositions
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
    • B01J37/02—Impregnation, coating or precipitation
    • B01J37/0215—Coating
    • B01J37/0225—Coating of metal substrates
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
    • B01J37/02—Impregnation, coating or precipitation
    • B01J37/024—Multiple impregnation or coating
    • B01J37/0242—Coating followed by impregnation
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL-COMBUSTION ENGINES
    • F01N13/00—Exhaust or silencing apparatus characterised by constructional features
    • F01N13/009—Exhaust or silencing apparatus characterised by constructional features having two or more separate purifying devices arranged in series
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL-COMBUSTION ENGINES
    • F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
    • F01N3/10—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust
    • F01N3/24—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by constructional aspects of converting apparatus
    • F01N3/28—Construction of catalytic reactors
    • F01N3/2803—Construction of catalytic reactors characterised by structure, by material or by manufacturing of catalyst support
    • F01N3/2807—Metal other than sintered metal
    • F01N3/281—Metallic honeycomb monoliths made of stacked or rolled sheets, foils or plates
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2255/00—Catalysts
    • B01D2255/10—Noble metals or compounds thereof
    • B01D2255/102—Platinum group metals
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2279/00—Filters adapted for separating dispersed particles from gases or vapours specially modified for specific uses
    • B01D2279/30—Filters adapted for separating dispersed particles from gases or vapours specially modified for specific uses for treatment of exhaust gases from IC Engines
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D46/00—Filters or filtering processes specially modified for separating dispersed particles from gases or vapours
    • B01D46/24—Particle separators, e.g. dust precipitators, using rigid hollow filter bodies
    • B01D46/2403—Particle separators, e.g. dust precipitators, using rigid hollow filter bodies characterised by the physical shape or structure of the filtering element
    • B01D46/2418—Honeycomb filters
    • B01D46/2451—Honeycomb filters characterized by the geometrical structure, shape, pattern or configuration or parameters related to the geometry of the structure
    • B01D46/248—Structures comprising laminated bodies or discs
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D46/00—Filters or filtering processes specially modified for separating dispersed particles from gases or vapours
    • B01D46/24—Particle separators, e.g. dust precipitators, using rigid hollow filter bodies
    • B01D46/2403—Particle separators, e.g. dust precipitators, using rigid hollow filter bodies characterised by the physical shape or structure of the filtering element
    • B01D46/2418—Honeycomb filters
    • B01D46/2451—Honeycomb filters characterized by the geometrical structure, shape, pattern or configuration or parameters related to the geometry of the structure
    • B01D46/2482—Thickness, height, width, length or diameter
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
    • B01J23/54—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
    • B01J23/56—Platinum group metals
    • B01J23/63—Platinum group metals with rare earths or actinides
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J35/00—Catalysts, in general, characterised by their form or physical properties
    • B01J35/50—Catalysts, in general, characterised by their form or physical properties characterised by their shape or configuration
    • B01J35/56—Foraminous structures having flow-through passages or channels, e.g. grids or three-dimensional [3D] monoliths
    • B01J35/57—Honeycombs
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL-COMBUSTION ENGINES
    • F01N2370/00—Selection of materials for exhaust purification
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL-COMBUSTION ENGINES
    • F01N2510/00—Surface coverings
    • F01N2510/06—Surface coverings for exhaust purification, e.g. catalytic reaction
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02A—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
    • Y02A50/00—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE in human health protection, e.g. against extreme weather
    • Y02A50/20—Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02T—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
    • Y02T10/00—Road transport of goods or passengers
    • Y02T10/10—Internal combustion engine [ICE] based vehicles
    • Y02T10/12—Improving ICE efficiencies

Definitions

  • the present invention relates to an exhaust-gas purifying catalyst. More specifically, it relates to an exhaust-gas purifying catalyst which is good in terms of the catalytic ignitability.
  • Exhaust-gas purifying systems using exhaust-gas purifying catalysts have been employed widely, because they can reduce the exhaust-gas emission remarkably, compared with the other measures, without applying so much load to internal combustion engines, such as automobile engines, which emit exhaust gases.
  • exhaust-gas purifying catalysts are made in the following manner.
  • a porous loading layer is formed on a surface of a catalyst support substrate which exhibits heat resistance.
  • the loading layer is composed of heat-resistant inorganic oxides, such as alumina.
  • a catalytic ingredient is loaded on the loading layer.
  • the exhaust-gas purifying catalysts convert nitrogen oxides (NO x ), hydrocarbons (HC) and carbon monoxide (CO), which are contained in exhaust gases, into unharmful nitrogen, carbon dioxide and water, respectively, by the action of catalytic ingredients.
  • Japanese Unexamined Patent Publication (KOKAI) No. 6-99,076 discloses a metallic support catalyst.
  • the metallic catalyst comprises two catalyst support substrates, a loading layer, and Pt and Rh.
  • the catalyst support substrates are fastened so as to be separated at an interval.
  • the loading layer is formed on a surface of the respective catalyst support substrates.
  • the Pt and Rh are loaded on the loading layer in an amount of 1.0 g and 0.2 g with respect to 1 L of an apparent volume of the catalyst support substrates, respectively.
  • Japanese Unexamined Patent Publication (KOKAI) No. 6-205,983 discloses an exhaust-gas purifying catalyst which comprises two catalyst support substrates, a loading layer, and Pt and Rh. Similarly, the catalyst support substrates are fastened so as to be separated at an interval. The loading layer is formed on a surface of the respective catalyst support substrates. The Pt and Rh are loaded on the loading layer.
  • the exhaust-gas purifying catalyst is characterized in that one of the catalytic ingredients, Pt, is loaded in a greater loading amount on an upstream side of the respective loading layers.
  • the Pt and Rh are loaded on an upstream portion of the loading layer formed on the upstream-side catalyst support substrate in an amount of 10.0 g and 0.3 g with respect to 1 L of an apparent volume of the upstream-side catalyst support substrate, respectively; and the Pt and Rh are loaded on the other portion of the loading layer formed on the upstream-side catalyst support substrate in an amount of 1.5 g and 0.3 g with respect to 1 L of an apparent volume of the upstream-side catalyst support substrate, respectively. Moreover, the Pt and Rh are loaded on the loading layer formed on the downstream-side catalyst support substrate in an amount of 10.0 g and 0.3 g with respect to 1 L of an apparent volume the downstream-side catalyst support substrate, respectively.
  • European Patent Application EP 1 136 115 A discloses also an exhaust gas purifying catalyst comprising two or more honeycomb-shaped supports disposed next one to the other in a mantle, both supports being provided with a catalytic layer.
  • the catalytic layer on the support upstream with respect to the flow of exhaust gases includes rhodium as a catalytic ingredient in an amount of up to 1 g with respect to 1 litre of the apparent volume of the upstream support.
  • the present invention has been developed in view of the aforementioned circumstances. It is therefore an object of the present invention to provide an exhaust-gas purifying catalyst which has such good ignition performance that it exhibits effective purifying activity even in a low temperature region, such as immediately after automotive engines are started.
  • the inventors of the present invention studied exhaust-gas purifying catalysts over and over again. As a result, they found out that it is possible to achieve the object when
  • an exhaust-gas purifying catalyst according to the present invention comprises:
  • the present exhaust-gas purifying catalyst comprises the catalytic layer which is disposed on a surface of the first honeycomb-shaped support and which includes Rh loaded in an amount of from 1.5 to 3g with respect to 1 L of an apparent volume of the first honeycomb-shaped support. Therefore, the present exhaust-gas purifying catalyst effects advantages that it exhibits not only good purifying performance but also upgraded ignition performance. Moreover, the present exhaust-gas purifying catalyst can be produced with a reduced loading amount of catalytic ingredient, because Rh gives exhaust-gas purifying catalysts better ignition performance with a less loading amount than platinum (Pt) and palladium (Pd) do.
  • Fig. 1 is a perspective view, which is cut away partially, for illustrating an arrangement of an exhaust-gas purifying catalyst according to Example No. 1 of the present invention.
  • Fig. 2 is a perspective view, which is cut away partially, for illustrating an arrangement of an exhaust-gas purifying catalyst according to Example No. 4 of the present invention.
  • Fig. 3 is a graph for illustrating the results of measurements for evaluating ignition performance and purifying performance which were exhibited by the exhaust-gas purifying catalysts according to Example Nos. 1 through 4 of the present invention as well as exhaust-gas purifying catalysts according Comparative Example Nos. 1 through 3.
  • the present exhaust-gas purifying catalyst comprises a mantle, two honeycomb-shaped supports, and a catalytic layer.
  • the mantel is composed of metals.
  • the metals forming the mantle heat-resistant metals are used which have been used in conventionally known pipe-shaped catalysts.
  • the heat-resistant metals it is possible to name stainless steel, for instance.
  • the two honeycomb-shaped supports are fastened in the mantle so as to be separated at intervals.
  • the honeycomb-shaped supports comprise a large number of cells which communicate one of the opposite ends of the honeycomb-shaped supports with the other one of them axially.
  • the honeycomb-shaped supports are disposed in the mantle so that the extension direction of cells coincides with the axial direction of the mantle.
  • the present exhaust-gas purifying catalyst comprises two or more independent component catalysts disposed in the mantle, because the two honeycomb-shaped supports are fastened in the mantle so as to be separated at intervals.
  • the honeycomb-shaped supports are composed of metals.
  • the honeycomb-shaped supports composed of metals enable the temperature of the respective independent component catalysts to rise quickly.
  • heat-resistant metals are used.
  • the heat-resistant metals it is possible to name stainless steel, for instance.
  • the catalytic layer is disposed on a surface of the respective honeycomb-shaped supports, and comprises a loading layer and a catalytic ingredient.
  • the loading layer is formed on a surface of the respective honeycomb-shaped supports.
  • the catalytic ingredient is loaded on the loading layer.
  • the catalytic layer purifies exhaust gases upon contacting with them.
  • the catalytic layer can comprise the same loading layer and catalytic ingredient as those of conventionally known exhaust-gas purifying catalysts.
  • the loading layer it is possible to use loading layers formed of heat-resistant inorganic oxides, such as alumina.
  • the loading layer can further comprise conventionally known additives, such as ceria and zirconia, dispersed therein.
  • the catalytic ingredient it is possible to use Pt, Pd or Rh.
  • the two honeycomb-shaped supports comprise a first honeycomb-shaped support, and a second honeycomb-shaped support.
  • the first honeycomb-shaped support is disposed on a most upstream side of the mantle with respect to a flow of exhaust gases.
  • the second honeycomb-shaped support is disposed next to the first honeycomb-shaped support on a downstream side of the mantle with respect to the flow of exhaust gases.
  • the catalytic layer disposed on a surface of the first honeycomb-shaped support includes at least Rh as the catalytic ingredient in a loading amount of from 1.5 to 3g with respect to 1 L of an apparent volume of the first honeycomb-shaped support.
  • the catalytic layer usually includes Rh in a loading amount of from 0.2 to 0.4 g approximately with respect to 1 L of an apparent volume of the support.
  • Rh is loaded in an amount of from 1.5 to 3g with respect to 1 L of an apparent volume of the first honeycomb-shaped support, a loading amount far greater than the conventional loading amount.
  • a first independent component catalyst formed on a surface of the first honeycomb-shaped support is upgraded in terms of the ignition performance and purifying performance, because the most-upstream-side catalytic layer includes Rh abundantly. Note that Rh produces better ignition performance with a less loading amount than Pt and Pd do.
  • Rh gives the present exhaust-gas purifying catalyst the advantage better with reduced noble metal consumption than both Pt and Pd are used.
  • the most-upstream-side catalytic layer includes Rh in a loading amount of from 1.5 to 3g, with respect to 1 L of an apparent volume of the first honeycomb-shaped support.
  • the two or more honeycomb-shaped supports are fastened in the mantle, and the catalytic layer is formed on the respective honeycomb-shaped supports. That is, the present exhaust-gas purifying catalyst comprises two or more independent component catalysts.
  • the quantity of independent component catalysts can be two or more.
  • the quantity of independent component catalysts can preferably be no more than two, because the more the quantity of independent component catalysts is the higher the production cost goes up.
  • the most-upstream-side catalytic layer can preferably further include one or more catalytic ingredients loaded thereon, in addition to Rh.
  • the loading amount of catalytic ingredients other than Rh is not limited in particular.
  • the loading amount can be arranged to such amounts that the catalytic ingredients other than Rh are loaded on conventional exhaust-gas purifying catalysts.
  • Pt and Pd can be loaded on the most-upstream-side catalytic layer in an amount of from 0.5 to 2.0 g and from 0.5 to 2.0 g, respectively, with respect to 1 L of an apparent volume of the first honeycomb-shaped support.
  • the catalytic layer disposed on a surface of the other honeycomb-shaped support of the two honeycomb-shaped supports (i.e., the two honeycomb-shaped supports excepting the first honeycomb-shaped support), can preferably include one or more catalytic ingredients loaded thereon.
  • the loading amount of catalytic ingredients is not limited in particular. However, when loading Rh on the catalytic layer disposed on a surface the honeycomb-shaped support other than the first honeycomb-shaped support, the Rh loading amount can preferably be arranged so that it is less than the Rh loading amount on the catalytic layer disposed on the first honeycomb-shaped support.
  • the catalytic layer disposed on the surface of the honeycomb-shaped support excepting the first honeycomb-shaped support can preferably include Rh as the catalytic ingredient in a loading amount less than that of the catalytic layer disposed on the first honeycomb-shaped support by a factor of from 0.1 to 0.7, further preferably from 0.4 to 0.6.
  • the quantity of the honeycomb-shaped catalysts excepting the first honeycomb-shaped support is more than two, it is possible to appropriately change the loading amount of the catalytic ingredient on each of the catalytic layers, disposed on the honeycomb-shaped catalysts excepting the first honeycomb-shaped support, respectively.
  • the loading amount of the catalytic ingredient on the catalytic layer, disposed on a surface of each of the honeycomb-shaped supports excepting the first honeycomb-shaped support can be arranged to such an amount that the catalytic ingredient is loaded on conventional exhaust-gas purifying catalysts.
  • Pt, Pd and Rh can be loaded on the catalytic layer, disposed on a surface of the honeycomb-shaped support excepting the first honeycomb-shaped support, in an amount of from 0.5 to 2.0 g, from 0.5 to 2.0 g, and from 0.2 to 0.5 g, respectively, with respect to 1 L of an apparent volume of the honeycomb-shaped support excepting the first honeycomb-shaped support.
  • the first honeycomb-shaped support can preferably have an axial length of from 10 to 30 mm.
  • the first independent component catalyst is upgraded in terms of the ignition performance. That is, the temperature increment rate of the first honeycomb support and that of the most-upstream-side catalytic layer surge when the first honeycomb-shaped support is shortened axially.
  • lengthening the axial length of the first honeycomb-shaped support results in a sharp increase in the production cost when loading Rh on the most-upstream-side catalytic layer. The shorter the axial length of the first honeycomb-shaped support the more preferable it is in view of the ignition performance.
  • the axial length of the first honeycomb-shaped support is less than 10 mm, the exhaust-gas blow-by (or exhaust-gas leakage) has occurred to degrade the ignition performance of resulting exhaust-gas purifying catalysts. Moreover, when the axial length of the first honeycomb-shaped support is less than 10 mm, it is difficult to manufacture such honeycomb-shaped supports. Note that the axial length of the first honeycomb-shaped support can further preferably be from 15 to 25 mm.
  • a summed axial length of the honeycomb-shaped support excepting the first honeycomb-shaped support can preferably be longer than that of the first honeycomb-shaped support.
  • the present exhaust-gas purifying catalyst has a catalytic layer with a sufficient length as a whole so that it can secure satisfactory exhaust-gas purifying performance.
  • An axial length of the second honeycomb-shaped support disposed next to the first honeycomb-shaped support can preferably be longer than that of the first honeycomb-shaped support.
  • the independent component catalyst formed on the second honeycomb-shaped support comprises the catalytic layer whose axial length is longer than that of the catalytic layer of the first independent component catalyst formed on the first honeycomb-shaped support.
  • the present exhaust-gas purifying catalyst can show enhanced exhaust-gas purifying performance.
  • the axial length of the second honeycomb-shaped support disposed next to the first honeycomb-shaped support can further preferably be longer than that of the first honeycomb-shaped support by from 20 to 150 mm, furthermore preferably from 40 to 120 mm.
  • the interval between the first honeycomb-shaped support and the second honeycomb-shaped support disposed next to the first honeycomb-shaped support falls in a range of from 5 to 50 mm.
  • the present exhaust-gas purifying catalyst can show not only high ignition performance but also upgraded exhaust-gas purifying performance.
  • the interval between the first honeycomb-shaped support and the second honeycomb-shaped support is less than 5 mm, the two independent component catalysts formed on the two honeycomb-shaped supports are disposed so closely that the turbulence of exhaust gases are less likely to occur between the two independent component catalysts. Accordingly, the overall exhaust-gas purifying efficiency might degrade.
  • the second independent component catalyst formed on the second honeycomb-shaped support is separated so away from the first independent component catalyst formed on the first honeycomb-shaped support that the second independent component catalyst might not utilize the enhanced ignition performance, the advantage produced by the first independent component catalyst, effectively. Consequently, the effective performance as an exhaust-gas purifying catalyst might degrade as a whole.
  • the interval between the first honeycomb-shaped support and the second honeycomb-shaped support is too long, the resulting exhaust-gas purifying catalysts themselves become so long that their boardability onto vehicles might deteriorate.
  • the interval between the first honeycomb-shaped support and the second honeycomb-shaped support disposed next to the first honeycomb-shaped support can further preferably fall in a range of from 10 to 30 mm.
  • the present exhaust-gas purifying catalyst can be arranged in the same manner as conventionally known exhaust-gas purifying catalysts, except that two or more independent component catalysts are formed in a mantle; and that one of the independent component catalysts, disposed on a first honeycomb-shaped support positioned on a most upstream side of the mantle with respect to a flow of exhaust gases, includes Rh as a catalytic ingredient in a loading amount of from 1.5 to 3g with respect to 1 L of an apparent volume of the first honeycomb-shaped support.
  • the production process of the present exhaust-gas purifying catalyst is not limited in particular.
  • the present exhaust-gas purifying catalyst can be produced in the following manner, for example.
  • a honeycomb-shaped support can be manufactured in the following manner, for instance.
  • a corrugated sheet is formed by bending a strip-shaped metallic sheet.
  • the resulting corrugated sheet is laminated with a strip-shaped flat metallic sheet.
  • the laminated corrugated sheet and flat sheet are wound as a roll.
  • the wound laminate is cut perpendicularly to the axial direction to a predetermined axial length.
  • the resultant honeycomb-shaped supports are fitted into a mantle.
  • the mantle comprises a pipe which has been cut to a predetermined axial length in advance. Then, the honeycomb-shaped supports are fastened in the mantle by brazing.
  • a slurry for forming a loading layer is coated on a surface of the honeycomb-shaped supports which are fastened in the mantle. After drying and calcining the slurry, a catalytic ingredient comprising Rh is loaded on the resulting loading layer in the same manner as conventional exhaust-gas purifying catalysts.
  • a circle-shaped continuous pipe was prepared which was composed of SUS436L as per Japanese Industrial Standard (JIS).
  • JIS Japanese Industrial Standard
  • the pipe had a thickness of 1.5 mm, an inside diameter of 50.5 mm, and an outside diameter of 53.5 mm.
  • the pipe was cut to an axial length of 140 mm to manufacture a mantle.
  • a cylindrical upstream-side honeycomb-shaped support which was composed of a high heat-resistance stainless steel.
  • the high heat-resistance stainless steel comprised 20% by weight of Cr, 5% by weight of Al, and the balance of Fe and inevitable impurities.
  • the upstream-side honeycomb-shaped support comprised cells in an amount of 31 cells/cm 2 (or 200 cells/inch 2 approximately), and had a diameter of 50.5 mm and an axial length of 20 mm. Note that the present first honeycomb-shaped support includes the upstream-side honeycomb-shaped support.
  • a cylindrical downstream-side honeycomb-shaped support was likewise manufactured which was composed of the high heat-resistance stainless steel.
  • the downstream-side honeycomb-shaped support comprised cells in an amount of 31 cells/cm 2 (or 200 cells/inch 2 approximately), and had a diameter of 50.5 mm and an axial length of 100 mm.
  • the present second honeycomb-shaped support includes the downstream-side honeycomb-shaped support.
  • the upstream-side honeycomb-shaped support and the downstream-side honeycomb-shaped support were manufactured in the following manner. Two strip-shaped sheets were prepared whose thickness was 100 ⁇ m, and were processed into a flat sheet and a corrugated sheet, respectively. The flat sheet and the corrugated sheet were laminated. Then, the laminated flat sheet and corrugated sheet were wound as a roll to manufacture the upstream-side honeycomb-shaped support and downstream-side honeycomb-shaped support.
  • the upstream-side honeycomb-shaped support was fitted into the mantle through one of the opposite-end openings of the mantle (hereinafter referred to as a "front-end opposite opening").
  • front-end opposite surface of the upstream-side honeycomb-shaped support was flush with the front-end opposite surface of the mantle when completing the fitting of the upstream-side honeycomb-shaped support into the mantle.
  • downstream-side honeycomb-shaped support was fitted into the mantle through the other one of the opposite-end openings of the mantle (hereinafter referred to as a "rear-end opposite opening”).
  • the rear-end opposite surface of the downstream-side honeycomb-shaped support was flush with the rear-end opposite surface of the mantle when completing the fitting of the downstream-side honeycomb-shaped support into the mantle.
  • the upstream-side and downstream honeycomb-shaped supports were fastened in the mantle by brazing in the following manner.
  • the fastening by brazing was carried out using a heat-resistant Ni-based brazing alloy.
  • the mantle into which the upstream-side and downstream-side honeycomb-shaped supports were fitted was heated to a high temperature and held thereat in a vacuum atmosphere.
  • the used brazing alloy comprised Cr in an amount of 18% by weight, Si in an amount of 10% by weight, and the balance of Ni and inevitable impurities.
  • alumina Al 2 O 3
  • ceria CeO 2
  • ZrO 2 zirconia
  • a binder 5 parts by weight of water.
  • the raw materials were mixed uniformly to prepare a slurry.
  • the resulting slurry was coated on a surface of the two honeycomb-shaped substrates, the upstream-side honeycomb-shaped support and the downstream-side honeycomb-shaped support, in a coating amount of 50 g/cm 2 , respectively.
  • the mantle into which the two honeycomb-shaped supports were fitted (hereinafter referred to as a "support assembly") was calcined at 500 °C for 1 hour.
  • an upstream-side loading layer and a downstream-side loading layer were formed on the upstream-side honeycomb-shaped support and the downstream-side honeycomb-shaped support, respectively.
  • a rhodium nitrate aqueous solution and a platinum nitrate aqueous solution were mixed to prepare a mixture aqueous solution.
  • the support assembly was immersed into the resultant mixture aqueous solution. After taking up the support assembly from the mixture aqueous solution and drying it, the support assembly was calcined. Note that the calcination was carried out by heating the support assembly at 300 °C for 1 hour.
  • Pt and Rh were loaded on the two loading layers, the upstream-side loading layer and the downstream-side loading layer, in a loading amount of 0.8 g and 0.16 g with respect to 1 L of an apparent volume of the two honeycomb-shaped supports, the upstream-side honeycomb-shaped support and the downstream-side honeycomb-shaped support, respectively.
  • a rhodium nitrate aqueous solution was further prepared. Only the upstream-side honeycomb-shaped support of the support assembly was immersed into the rhodium nitrate aqueous solution. After taking up the upstream-side honeycomb-shaped support of the support assembly from the rhodium nitrate aqueous solution and drying it, the support assembly was calcined. Note that the calcination was carried out by heating the support assembly at 300 °C for 1 hour. When the process was completed, Rh was further loaded on the upstream-side loading layer in an extra loading amount of 0.8 g with respect to 1 L of an apparent volume of the upstream-side honeycomb-shaped support. That is, Rh was loaded on the upstream-side loading layer in a total loading amount of 0.96 g with respect to 1 L of an apparent volume of the upstream-side honeycomb-shaped support.
  • FIG. 1 illustrates the arrangement of the exhaust-gas purifying catalyst according to Example No. 1.
  • the exhaust-gas purifying catalyst 1 according to Example No. 1 comprised the mantle 2, the upstream-side catalyst 3, and the downstream-side catalyst 4.
  • the upstream-side catalyst 3 was disposed in the mantle 2 on an upstream side with respect to a flow of exhaust gases; and the downstream-side catalyst 4 was disposed at a position where the upstream-end surface of the downstream-side catalyst 4 was positioned away from the downstream-end surface of the upstream-side catalyst 3 at an interval of 20 mm.
  • the upstream-end surface of the upstream-side catalyst 3 agreed with the upstream-end surface of the mantle 2; and the downstream-end surface of the downstream-side catalyst 4 agreed with the downstream-end surface of the mantle 2.
  • the upstream-side catalyst 3 comprised the upstream-side honeycomb-shaped support fastened to the mantle 2, and the upstream-side catalytic layer formed on a surface of the upstream-side honeycomb-shaped support
  • the downstream-side catalyst 4 comprised the downstream-side honeycomb-shaped support fastened to the mantle 2, and the downstream-side catalytic layer formed on a surface of the downstream-side honeycomb-shaped support.
  • the upstream-side catalytic layer comprised the upstream-side loading layer formed on a surface of the upstream-side honeycomb-shaped support, and Pt and Rh loaded on the upstream-side loading layer; and the downstream-side catalytic layer comprised the downstream-side loading layer formed on a surface of the downstream-side honeycomb-shaped support, and Pt and Rh loaded on the downstream-side loading layer.
  • Rh was loaded on the upstream-side loading layer in a loading amount of 0.96 g with respect to 1 L of an apparent volume of the upstream-side honeycomb-shaped support.
  • Table 1 summarizes the arrangement of the exhaust-gas purifying catalyst according to Example No. 1.
  • Table 1 summarizes the arrangement of the exhaust-gas purifying catalyst according to Example No. 1.
  • Table 1 summarizes the arrangement of the exhaust-gas purifying catalyst according to Example No. 1.
  • Table 1 summarizes the arrangement of the exhaust-gas purifying catalyst according to Example No. 1.
  • Table 1 summarizes the arrangement of the exhaust-gas purifying catalyst according to Example No. 1.
  • the component members were used whose material qualities and sizes were the same as those of the component members used in Example No. 1.
  • the two honeycomb-shaped supports, the upstream-side support and the downstream-side support, were fastened in the mantle to prepare the support assembly. Then, the upstream-side and downstream-side loading layers were formed on a surface of the two honeycomb-shaped supports, respectively.
  • a rhodium nitrate aqueous solution and a platinum nitrate aqueous solution were mixed to prepare a mixture aqueous solution.
  • the support assembly was immersed into the resultant mixture aqueous solution. After taking up the support assembly from the mixture aqueous solution and drying it, the support assembly was calcined. Note that the calcination was carried out by heating the support assembly at 300 °C for 1 hour.
  • Pt and Rh were loaded on the two loading layers, the upstream-side loading layer and the downstream-side loading layer, in a loading amount of 0.8 g and 0.16 g with respect to 1 L of an apparent volume of the two honeycomb-shaped supports, the upstream-side honeycomb-shaped support and the downstream-side honeycomb-shaped support, respectively.
  • a rhodium nitrate aqueous solution was further prepared. Only the upstream-side honeycomb-shaped support of the support assembly was immersed into the rhodium nitrate aqueous solution. After taking up the upstream-side honeycomb-shaped support of the support assembly from the rhodium nitrate aqueous solution and drying it, the support assembly was calcined. Note that the calcination was carried out by heating the support assembly at 300 °C for 1 hour. When the process was completed, Rh was further loaded on the upstream-side loading layer in an extra loading amount of 2.3 g with respect to 1 L of an apparent volume of the upstream-side honeycomb-shaped support. That is, Rh was loaded on the upstream-side loading layer in a total loading amount of 2.46 g with respect to 1 L of an apparent volume of the upstream-side honeycomb-shaped support.
  • the exhaust-gas purifying catalyst according to Example No. 2 comprised the mantle, the upstream-side catalyst, and the downstream-side catalyst.
  • the upstream-side catalyst was disposed in the mantle on an upstream side with respect to a flow of exhaust gases; and the downstream-side catalyst was disposed at a position where the upstream-end surface of the downstream-side catalyst was positioned away from the downstream-end surface of the upstream-side catalyst at an interval of 20 mm.
  • the upstream-end surface of the upstream-side catalyst agreed with the upstream-end surface of the mantle; and the downstream-end surface of the downstream-side catalyst agreed with the downstream-end surface of the mantle.
  • the upstream-side catalyst comprised the upstream-side honeycomb-shaped support fastened to the mantle, and the upstream-side catalytic layer formed on a surface of the upstream-side honeycomb-shaped support; and the downstream-side catalyst comprised the downstream-side honeycomb-shaped support fastened to the mantle, and the downstream-side catalytic layer formed on a surface of the downstream-side honeycomb-shaped support.
  • the upstream-side catalytic layer comprised the upstream-side loading layer formed on a surface of the upstream-side honeycomb-shaped support, and Pt and Rh loaded on the upstream-side loading layer; and the downstream-side catalytic layer comprised the downstream-side loading layer formed on a surface of the downstream-side honeycomb-shaped support, and Pt and Rh loaded on the downstream-side loading layer.
  • Rh was loaded on the upstream-side loading layer in a loading amount of 2.46 g with respect to 1 L of an apparent volume of the upstream-side honeycomb-shaped support.
  • Table 1 above summarizes the arrangement of the exhaust-gas purifying catalyst according to Example No. 2 as well.
  • the component members were used whose material qualities and sizes were the same as those of the component members used in Example No. 1.
  • the two honeycomb-shaped supports, the upstream-side support and the downstream-side support, were fastened in the mantle to prepare the support assembly. Then, the upstream-side and downstream-side loading layers were formed on a surface of the two honeycomb-shaped supports, respectively.
  • a rhodium nitrate aqueous solution and a palladium nitrate aqueous solution were mixed to prepare a mixture aqueous solution.
  • the support assembly was immersed into the resultant mixture aqueous solution. After taking up the support assembly from the mixture aqueous solution and drying it, the support assembly was calcined. Note that the calcination was carried out by heating the support assembly at 300 °C for 1 hour.
  • Pd and Rh were loaded on the two loading layers, the upstream-side loading layer and the downstream-side loading layer, in a loading amount of 0.8 g and 0.16 g with respect to 1 L of an apparent volume of the two honeycomb-shaped supports, the upstream-side honeycomb-shaped support and the downstream-side honeycomb-shaped support, respectively.
  • a rhodium nitrate aqueous solution was further prepared. Only the upstream-side honeycomb-shaped support of the support assembly was immersed into the rhodium nitrate aqueous solution. After taking up the upstream-side honeycomb-shaped support of the support assembly from the rhodium nitrate aqueous solution and drying it, the support assembly was calcined. Note that the calcination was carried out by heating the support assembly at 300 °C for 1 hour. When the process was completed, Rh was further loaded on the upstream-side loading layer in an extra loading amount of 0.8 g with respect to 1 L of an apparent volume of the upstream-side honeycomb-shaped support. That is, Rh was loaded on the upstream-side loading layer in a total loading amount of 0.96 g with respect to 1 L of an apparent volume of the upstream-side honeycomb-shaped support.
  • the exhaust-gas purifying catalyst according to Example No. 3 comprised the mantle, the upstream-side catalyst, and the downstream-side catalyst.
  • the upstream-side catalyst was disposed in the mantle on an upstream side with respect to a flow of exhaust gases; and the downstream-side catalyst was disposed at a position where the upstream-end surface of the downstream-side catalyst was positioned away from the downstream-end surface of the upstream-side catalyst at an interval of 20 mm.
  • the upstream-end surface of the upstream-side catalyst agreed with the upstream-end surface of the mantle; and the downstream-end surface of the downstream-side catalyst agreed with the downstream-end surface of the mantle.
  • the upstream-side catalyst comprised the upstream-side honeycomb-shaped support fastened to the mantle, and the upstream-side catalytic layer formed on a surface of the upstream-side honeycomb-shaped support; and the downstream-side catalyst comprised the downstream-side honeycomb-shaped support fastened to the mantle, and the downstream-side catalytic layer formed on a surface of the downstream-side honeycomb-shaped support.
  • the upstream-side catalytic layer comprised the upstream-side loading layer formed on a surface of the upstream-side honeycomb-shaped support, and Pd and Rh loaded on the upstream-side loading layer; and the downstream-side catalytic layer comprised the downstream-side loading layer formed on a surface of the downstream-side honeycomb-shaped support, and Pd and Rh loaded on the downstream-side loading layer.
  • Rh was loaded on the upstream-side loading layer in a loading amount of 0.96 g with respect to 1 L of an apparent volume of the upstream-side honeycomb-shaped support.
  • Table 1 above summarizes the arrangement of the exhaust-gas purifying catalyst according to Example No. 3 as well.
  • a circle-shaped continuous pipe was prepared which was composed of SUS436L as per Japanese Industrial Standard (JIS).
  • JIS Japanese Industrial Standard
  • the pipe had a thickness of 1.5 mm, an inside diameter of 50.5 mm, and an outside diameter of 53.5 mm.
  • the pipe was cut to an axial length of 140 mm to manufacture a mantle.
  • a cylindrical upstream-side honeycomb support was manufactured which was composed of the above-described high heat-resistance stainless steel.
  • the upstream-side honeycomb-shaped support comprised cells in an amount of 31 cells/cm 2 (or 200 cells/inch 2 approximately), and had a diameter of 50.5 mm and an axial length of 20 mm. Note that the present first honeycomb-shaped support includes the upstream-side honeycomb-shaped support.
  • a cylindrical intermediate honeycomb-shaped support was likewise manufactured which was composed of the high heat-resistance stainless steel.
  • the intermediate honeycomb support comprised cells in an amount of 31 cells/cm 2 (or 200 cells/inch 2 approximately), and had a diameter of 50.5 mm and an axial length of 40 mm. Note that the present second honeycomb-shaped support includes the intermediate honeycomb-shaped support.
  • a cylindrical downstream-side honeycomb-shaped support was likewise manufactured which was composed of the high heat-resistance stainless steel.
  • the downstream-side honeycomb-shaped support comprised cells in an amount of 31 cells/cm 2 (or 200 cells/inch 2 approximately), and had a diameter of 50.5 mm and an axial length of 40 mm.
  • the intermediate honeycomb-shaped support was fitted into the mantle through one of the opposite-end openings of the mantle (hereinafter referred to as a "front-end opposite opening").
  • the intermediate honeycomb-shaped support was fitted into the mantle until the front-end opposite surface of the intermediate honeycomb-shaped support was positioned away from the front-end opposite surface of the mantle by a distance of 40 mm.
  • the upstream-side honeycomb-shaped support was fitted into the mantle through the front-end opposite opening. Note that the front-end opposite surface of the upstream-side honeycomb-shaped support was flush with the front-end opposite surface of the mantle when completing the fitting of the upstream-side honeycomb-shaped support into the mantle.
  • downstream-side honeycomb-shaped support was fitted into the mantle through the other one of the opposite-end openings of the mantle (hereinafter referred to as a "rear-end opposite opening").
  • rear-end opposite surface of the downstream-side honeycomb-shaped support was flush with the rear-end opposite surface of the mantle when completing the fitting of the downstream-side honeycomb-shaped support into the mantle.
  • the intermediate honeycomb-shaped support was disposed at a position where the front-end opposite opening of the intermediate honeycomb-shaped support was positioned away from the rear-end opposite opening of the upstream-side honeycomb-shaped support by a distance of 20 mm; and the downstream-side honeycomb-shaped support was disposed at a position where the front-end opposite opening of the downstream-side honeycomb-shaped support was positioned away from the rear-end opposite opening of the intermediate honeycomb-shaped support by a distance of 20 mm.
  • the mantle was fastened to the upstream-side, intermediate and downstream honeycomb-shaped supports which were fitted into the mantle by brazing in the following manner.
  • the fastening by brazing was carried out using a heat-resistant Ni-based brazing alloy.
  • the heat-resistant Ni-brazing alloy After applying the heat-resistant Ni-brazing alloy onto an inner peripheral surface of the mantle and onto an outer peripheral surface of the upstream-side, intermediate and downstream honeycomb-shaped supports, the mantle into which the upstream-side, intermediate and downstream-side honeycomb-shaped supports were fitted was heated to a high temperature and held thereat in a vacuum atmosphere.
  • the used brazing alloy comprised Cr in an amount of 18% by weight, Si in an amount of 10% by weight, and the balance of Ni and inevitable impurities.
  • alumina Al 2 O 3
  • ceria CeO 2
  • ZrO 2 zirconia
  • a binder 5 parts by weight of water.
  • the raw materials were mixed uniformly to prepare a slurry.
  • the resulting slurry was coated on a surface of the three honeycomb-shaped substrates, the upstream-side honeycomb-shaped support, the intermediate honeycomb-shaped support and the downstream-side honeycomb-shaped support, in a coating amount of 50 g/cm 2 , respectively.
  • the support assembly was calcined at 500 °C for 1 hour.
  • an upstream-side loading layer, an intermediate loading layer and a downstream-side loading layer were formed on the upstream-side honeycomb-shaped support, the intermediate honeycomb-shaped support and the downstream-side honeycomb-shaped support, respectively.
  • a rhodium nitrate aqueous solution and a platinum nitrate aqueous solution were mixed to prepare a mixture aqueous solution.
  • the support assembly was immersed into the resultant mixture aqueous solution. After taking up the support assembly from the mixture aqueous solution and drying it, the support assembly was calcined. Note that the calcination was carried out by heating the support assembly at 300 °C for 1 hour.
  • Pt and Rh were loaded on the three loading layers, the upstream-side loading layer, the intermediate loading layer and the downstream-side loading layer, in a loading amount of 0.8 g and 0.16 g with respect to 1 L of an apparent volume of the three honeycomb-shaped supports, the upstream-side honeycomb-shaped support, the intermediate honeycomb-shaped support and the downstream-side honeycomb-shaped support, respectively.
  • a rhodium nitrate aqueous solution was further prepared. Only the upstream-side honeycomb-shaped support of the support assembly was immersed into the rhodium nitrate aqueous solution. After taking up the upstream-side honeycomb-shaped support of the support assembly from the rhodium nitrate aqueous solution and drying it, the support assembly was calcined. Note that the calcination was carried out by heating the support assembly at 300 °C for 1 hour. When the process was completed, Rh was further loaded on the upstream-side loading layer in an extra loading amount of 0.8 g with respect to 1 L of an apparent volume of the upstream-side honeycomb-shaped support. That is, Rh was loaded on the upstream-side loading layer in a total loading amount of 0.96 g with respect to 1 L of an apparent volume of the upstream-side honeycomb-shaped support.
  • FIG. 2 illustrates the arrangement of the exhaust-gas purifying catalyst according to Example No. 4.
  • the exhaust-gas purifying catalyst 1' comprised the mantle 2', the upstream-side catalyst 3', the intermediate catalyst 5, and the downstream-side catalyst 4'.
  • the upstream-side catalyst 3' was disposed in the mantle 2' on an upstream side with respect to a flow of exhaust gases;
  • the intermediate catalyst 5 was disposed at a position where the upstream-end surface of the intermediate catalyst 5 was positioned away from the downstream-end surface of the upstream-side catalyst 3' at an interval of 20 mm;
  • the downstream-side catalyst 4' was disposed at a position where the upstream-end surface of the downstream-side catalyst 4' was positioned away from the downstream-end surface of the intermediate catalyst 5 at an interval of 20 mm.
  • the upstream-end surface of the upstream-side catalyst 3' agreed with the upstream-end surface of the mantle 2'; and the downstream-end surface of the downstream-side catalyst 4' agreed with the downstream-end surface of the mantle 2'.
  • the upstream-side catalyst 3' comprised the upstream-side honeycomb-shaped support fastened to the mantle 2', and the upstream-side catalytic layer formed on a surface of the upstream-side honeycomb-shaped support;
  • the intermediate catalyst 5 comprised the intermediate honeycomb-shaped support fastened to the mantle 2', and the intermediate catalytic layer formed on a surface of the intermediate honeycomb-shaped support;
  • the downstream-side catalyst 4' comprised the downstream-side honeycomb-shaped support fastened to the mantle 2', and the downstream-side catalytic layer formed on a surface of the downstream-side honeycomb-shaped support.
  • the upstream-side catalytic layer comprised the upstream-side loading layer formed on a surface of the upstream-side honeycomb-shaped support, and Pt and Rh loaded on the upstream-side loading layer;
  • the intermediate catalytic layer comprised the intermediate loading layer formed on a surface of the intermediate honeycomb-shaped support, and Pt and Rh loaded on the intermediate loading layer;
  • the downstream-side catalytic layer comprised the downstream-side loading layer formed on a surface of the downstream-side honeycomb-shaped support, and Pt and Rh loaded on the downstream-side loading layer.
  • Rh was loaded on the upstream-side loading layer in a loading amount of 0.96 g with respect to 1 L of an apparent volume of the upstream-side honeycomb-shaped support.
  • Table 1 above summarizes the arrangement of the exhaust-gas purifying catalyst according to Example No. 4 as well.
  • a circle-shaped continuous pipe was prepared which was composed of SUS436L as per Japanese Industrial Standard (JIS).
  • JIS Japanese Industrial Standard
  • the pipe had a thickness of 1.5 mm, an inside diameter of 50.5 mm, and an outside diameter of 53.5 mm.
  • the pipe was cut to an axial length of 120 mm to manufacture a mantle.
  • honeycomb-shaped support which was composed of the above-described high heat-resistance stainless steel.
  • the honeycomb-shaped support comprised cells in an amount of 31 cells/cm 2 (or 200 cells/inch 2 approximately), and had a diameter of 50.5 mm and an axial length of 120 mm.
  • honeycomb-shaped support was manufactured in the following manner. Two strip-shaped sheets were prepared whose thickness was 100 ⁇ m, and were processed into a flat sheet and a corrugated sheet, respectively. The flat sheet and the corrugated sheet were laminated. Then, the laminated flat sheet and corrugated sheet were wound as a roll to manufacture the honeycomb-shaped support.
  • the honeycomb-shaped support was fitted into the mantle through one of the opposite-end openings of the mantle (hereinafter referred to as a "front-end opposite opening"). Note that the front-end opposite surface of the honeycomb-shaped support was flush with the front-end opposite surface of the mantle when completing the fitting of the honeycomb-shaped support into the mantle.
  • the honeycomb-shaped support was fastened in the mantle by brazing in the following manner.
  • the fastening by brazing was carried out using a heat-resistant Ni-based brazing alloy.
  • the mantle into which the honeycomb-shaped support was fitted was heated to a high temperature and held thereat in a vacuum atmosphere.
  • the used brazing alloy comprised Cr in an amount of 18% by weight, Si in an amount of 10% by weight, and the balance of Ni and inevitable impurities.
  • alumina Al 2 O 3
  • ceria CeO 2
  • ZrO 2 zirconia
  • a binder 5 parts by weight of water.
  • the raw materials were mixed uniformly to prepare a slurry.
  • the resulting slurry was coated on a surface of the honeycomb-shaped support in a coating amount of 50 g/cm 2 . After drying the coated slurry, the support assembly was calcined at 500 °C for 1 hour. Thus, a loading layer was formed on the honeycomb-shaped support.
  • a rhodium nitrate aqueous solution and a platinum nitrate aqueous solution were mixed to prepare a mixture aqueous solution.
  • the support assembly was immersed into the resultant mixture aqueous solution. After taking up the support assembly from the mixture aqueous solution and drying it, the support assembly was calcined. Note that the calcination was carried out by heating the support assembly at 300 °C for 1 hour.
  • Pt and Rh were loaded on the loading layer in a loading amount of 0.8 g and 0.3 g with respect to 1 L of an apparent volume of the honeycomb-shaped support.
  • the exhaust-gas purifying catalyst according to Comparative Example No. 1 comprised the mantle, and the single honeycomb-shaped support.
  • the single honeycomb-shaped support was fastened in the mantle.
  • a catalytic layer was formed on a surface of the single honeycomb-shaped support.
  • the catalytic layer comprised the loading layer formed on a surface of the single honeycomb-shaped support, and Pt and Rh loaded on the loading layer.
  • the axial length of the single honeycomb-shaped support, used in the exhaust-gas purifying catalyst according to Comparative Example No. 1 was equal to a sum of the axial length of the upstream-side honeycomb-shaped support and the axial length of the downstream-side honeycomb-shaped support, used in the exhaust-gas purifying catalyst according to Example No. 1.
  • Table 1 above summarizes the arrangement of the exhaust-gas purifying catalyst according to Comparative Example No. 1 as well.
  • the component members were used whose material qualities and sizes were the same as those of the component members used in Example No. 1.
  • the two honeycomb-shaped supports, the upstream-side support and the downstream-side support, were fastened in the mantle to prepare the support assembly. Then, the upstream-side and downstream-side loading layers were formed on a surface of the two honeycomb-shaped supports, respectively.
  • a rhodium nitrate aqueous solution and a platinum nitrate aqueous solution were mixed to prepare a mixture aqueous solution.
  • the support assembly was immersed into the resultant mixture aqueous solution. After taking up the support assembly from the mixture aqueous solution and drying it, the support assembly was calcined. Note that the calcination was carried out by heating the support assembly at 300 °C for 1 hour.
  • Pt and Rh were loaded on the two loading layers, the upstream-side loading layer and the downstream-side loading layer, in a loading amount of 0.8 g and 0.16 g with respect to 1 L of an apparent volume of the two honeycomb-shaped supports, the upstream-side honeycomb-shaped support and the downstream-side honeycomb-shaped support, respectively.
  • a palladium nitrate aqueous solution was further prepared. Only the upstream-side honeycomb-shaped support of the support assembly was immersed into the palladium nitrate aqueous solution. After taking up the upstream-side honeycomb-shaped support of the support assembly from the palladium nitrate aqueous solution and drying it, the support assembly was calcined. Note that the calcination was carried out by heating the support assembly at 300 °C for 1 hour. When the process was completed, Pd was further loaded on the upstream-side loading layer in a loading amount of 1.6 g with respect to 1 L of an apparent volume of the upstream-side honeycomb-shaped support.
  • the exhaust-gas purifying catalyst according to Comparative Example No. 2 comprised the mantle, the upstream-side catalyst, and the downstream-side catalyst.
  • the upstream-side catalyst was disposed in the mantle on an upstream side with respect to a flow of exhaust gases; and the downstream-side catalyst was disposed at a position where the upstream-end surface of the downstream-side catalyst was positioned away from the downstream-end surface of the upstream-side catalyst at an interval of 20 mm.
  • the upstream-end surface of the upstream-side catalyst agreed with the upstream-end surface of the mantle; and the downstream-end surface of the downstream-side catalyst agreed with the downstream-end surface of the mantle.
  • the upstream-side catalyst comprised the upstream-side honeycomb-shaped support fastened to the mantle, and the upstream-side catalytic layer formed on a surface of the upstream-side honeycomb-shaped support; and the downstream-side catalyst comprised the downstream-side honeycomb-shaped support fastened to the mantle, and the downstream-side catalytic layer formed on a surface of the downstream-side honeycomb-shaped support.
  • the upstream-side catalytic layer comprised the upstream-side loading layer formed on a surface of the upstream-side honeycomb-shaped support, and Pt, Rh and Pd loaded on the upstream-side loading layer; and the downstream-side catalytic layer comprised the downstream-side loading layer formed on a surface of the downstream-side honeycomb-shaped support, and Pt and Rh loaded on the downstream-side loading layer.
  • Rh was loaded on the upstream-side loading layer in a loading amount of 0.16 g with respect to 1 L of an apparent volume of the upstream-side honeycomb-shaped support.
  • Table 1 above summarizes the arrangement of the exhaust-gas purifying catalyst according to Comparative Example No. 2 as well.
  • the component members were used whose material qualities and sizes were the same as those of the component members used in Example No. 1.
  • the two honeycomb-shaped supports, the upstream-side support and the downstream-side support, were fastened in the mantle to prepare the support assembly. Then, the upstream-side and downstream-side loading layers were formed on a surface of the two honeycomb-shaped supports, respectively.
  • a rhodium nitrate aqueous solution and a platinum nitrate aqueous solution were mixed to prepare a mixture aqueous solution.
  • the support assembly was immersed into the resultant mixture aqueous solution. After taking up the support assembly from the mixture aqueous solution and drying it, the support assembly was calcined. Note that the calcination was carried out by heating the support assembly at 300 °C for 1 hour.
  • Pt and Rh were loaded on the two loading layers, the upstream-side loading layer and the downstream-side loading layer, in a loading amount of 0.8 g and 0.16 g with respect to 1 L of an apparent volume of the two honeycomb-shaped supports, the upstream-side honeycomb-shaped support and the downstream-side honeycomb-shaped support, respectively.
  • a platinum nitrate aqueous solution was further prepared. Only the upstream-side honeycomb-shaped support of the support assembly was immersed into the platinum nitrate aqueous solution. After taking up the upstream-side honeycomb-shaped support of the support assembly from the platinum nitrate aqueous solution and drying it, the support assembly was calcined. Note that the calcination was carried out by heating the support assembly at 300 °C for 1 hour. When the process was completed, Pt was further loaded on the upstream-side loading layer in an extra loading amount of 1.6 g with respect to 1 L of an apparent volume of the upstream-side honeycomb-shaped support. That is, Pt was loaded on the upstream-side loading layer in a total loading amount of 2.4 g with respect to 1 L of an apparent volume of the upstream-side honeycomb-shaped support.
  • the exhaust-gas purifying catalyst according to Comparative Example No. 3 comprised the mantle, the upstream-side catalyst, and the downstream-side catalyst.
  • the upstream-side catalyst was disposed in the mantle on an upstream side with respect to a flow of exhaust gases; and the downstream-side catalyst was disposed at a position where the upstream-end surface of the downstream-side catalyst was positioned away from the downstream-end surface of the upstream-side catalyst at an interval of 20 mm.
  • the upstream-end surface of the upstream-side catalyst agreed with the upstream-end surface of the mantle; and the downstream-end surface of the downstream-side catalyst agreed with the downstream-end surface of the mantle.
  • the upstream-side catalyst comprised the upstream-side honeycomb-shaped support fastened to the mantle, and the upstream-side catalytic layer formed on a surface of the upstream-side honeycomb-shaped support; and the downstream-side catalyst comprised the downstream-side honeycomb-shaped support fastened to the mantle, and the downstream-side catalytic layer formed on a surface of the downstream-side honeycomb-shaped support.
  • the upstream-side catalytic layer comprised the upstream-side loading layer formed on a surface of the upstream-side honeycomb-shaped support, and Pt and Rh loaded on the upstream-side loading layer; and the downstream-side catalytic layer comprised the downstream-side loading layer formed on a surface of the downstream-side honeycomb-shaped support, and Pt and Rh loaded on the downstream-side loading layer.
  • Pt and Rh were loaded on the upstream-side loading layer in a loading amount of 2.4 g and 0.16 g with respect to 1 L of an apparent volume of the upstream-side honeycomb-shaped support, respectively.
  • Table 1 above summarizes the arrangement of the exhaust-gas purifying catalyst according to Comparative Example No. 3 as well.
  • Example Nos. 1 through 4 and Comparative Example Nos. 1 through 3 were assembled with an exhaust system of an automotive engine testing bench equipped with an engine whose displacement was 2,000 c.c., respectively. Then, the engine was started to subject the exhaust-gas purifying catalysts to a durability test for 100 hours while running the engine at a revolving speed of 5,000 rpm and setting the inlet exhaust-gas temperature at 800 °C.
  • the respective exhaust-gas purifying catalysts which had been subjected to the durability test, were mounted on an exhaust system of an actual vehicle (e.g., a two-wheeled vehicle) equipped with a 4-stroke engine whose displacement was 0.4 L.
  • the engine was driven under the running conditions prescribed in ECE40 (or ISO6460), and exhaust gases emitted from the engine were passed through the exhaust-gas purifying catalysts.
  • ECE40 or ISO6460
  • the bag sampling was started in which the exhaust gases, which had passed through the exhaust-gas purifying catalysts and had been emitted therefrom, were collected. Note that the bag sampling was carried out in the following manner.
  • the comparison results were similar to those relating to the first bags.
  • the CO emission values in the exhaust gases emitted from the exhaust-gas purifying catalyst according to Example No. 2 was remarkably smaller value than the CO emission values in the exhaust gases emitted from the exhaust-gas purifying catalysts according to Example Nos. 1, 3 through 4 and Comparative Example Nos. 1 through 3.
  • a small CO emission value in exhaust gases collected in the second bag indicates that an exhaust-gas purifying catalyst is better in terms of the purifying performance, because the second bag collects exhaust gases emitted from engines in the third through sixth cycles of the ECE40 mode, that is, after the ignition. Therefore, it is understood that the exhaust-gas purifying catalyst according to Example No. 2 exhibited better exhaust-gas purifying performance.
  • exhaust-gas purifying catalyst according to Example No. 4 is an example which comprises two honeycomb-shaped supports in addition to the first honeycomb-shaped support.
  • the exhaust-gas purifying catalyst according to Example No. 2 was good in terms of the ignition performance and purifying performance.

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Claims (11)

  1. Catalyseur de purification des gaz d'échappement (1), comprenant :
    une enveloppe faite en métal résistant à la chaleur ;
    deux supports en nid-d'abeilles faite en métal résistant à la chaleur fixés dans l'enveloppe (2) de sorte à être séparés par intervalles, et comprenant un premier support en nid-d'abeilles (3) disposé sur un côté le plus en amont de l'enveloppe (2) par rapport à un flux de gaz d'échappement et un deuxième support en nid-d'abeilles (4) disposé à proximité du premier support en nid-d'abeilles sur un côté aval de l'enveloppe par rapport au flux de gaz d'échappement ; et
    une couche catalytique disposée sur une surface des supports respectifs en nid-d'abeilles, et comprenant une couche de charge formée sur une surface des supports respectifs en nid-d'abeilles (3, 4) et un ingrédient catalytique chargé sur la couche de charge, la couche catalytique disposée sur une surface du premier support en nid-d'abeilles (3) comprenant au moins du rhodium (Rh)
    en tant que l'ingrédient catalytique dans une quantité de charge de 1,5 à 3 g par rapport à un volume apparent d'un 1 litre u premier support en nid-d'abeilles (3) ; et
    dans lequel l'intervalle séparant le premier support en nid-d'abeilles du deuxième support en nid-d'abeilles disposé à proximité du premier support en nid-d'abeilles mesure de 5 à 50 mm.
  2. Catalyseur de purification des gaz d'échappement (1) selon la revendication 1, dans lequel le premier support en nid-d'abeilles (3) a une longueur axiale allant de 10 à 30 mm.
  3. Catalyseur de purification des gaz d'échappement (1) selon la revendication 1, dans lequel une longueur axiale additionnée des supports en nid-d'abeilles (3, 4) à l'exception du premier support en nid-d'abeilles (3) est supérieure à celle du premier support en nid-d'abeilles (3).
  4. Catalyseur de purification des gaz d'échappement (1) selon la revendication 1, dans lequel une longueur axiale du deuxième support en nid-d'abeilles (4) disposé à proximité du premier support en nid-d'abeilles (3) est supérieure à celle du premier support en nid-d'abeilles 3).
  5. Catalyseur de purification des gaz d'échappement (1) selon la revendication 4, dans lequel la longueur axiale du deuxième support en nid-d'abeilles (4) est supérieure à celle du premier support en nid-d'abeilles (3) d'environ 20 à 150 mm.
  6. Catalyseur de purification des gaz d'échappement (1) selon la revendication 1, dans lequel la couche catalytique disposée sur la surface du premier support en nid-d'abeilles (3) comprend en outre un élément choisi parmi le groupe comprenant le platine (Pt) et le palladium (Pd) en tant que l'ingrédient catalytique selon un rapport de charge allant de 0,5 à 2,0 g et de 0,5 à 2,0 g respectivement, par rapport à 1 litre d'un volume appareil du premier support en nid-d'abeilles (3).
  7. Catalyseur de purification des gaz d'échappement (1) selon la revendication 1, dans lequel la couche catalytique disposée sur la surface des supports en nid-d'abeilles (3, 4) à l'exception du premier support en nid-d'abeilles (3) comprend du Rh en tant que l'ingrédient catalytique, dans une quantité de charge inférieure à celle de la couche catalytique disposée sur le premier support en nid-d'abeilles (3).
  8. Catalyseur de purification des gaz d'échappement (1) selon la revendication 7, dans lequel la couche catalytique disposée sur la surface des supports en nid-d'abeilles (3, 4) à l'exception du premier support en nid-d'abeilles (3) comprend du Rh en tant que l'ingrédient catalytique, dans une quantité de charge inférieure d'un facteur allant de 0,1 à 0,7 à celui de la couche catalytique disposée sur le premier support en nid-d'abeilles (3).
  9. Catalyseur de purification des gaz d'échappement (1) selon la revendication 7, dans lequel la couche catalytique disposée sur la surface des supports en nid-d'abeilles (3, 4) à l'exception du premier support en nid-d'abeilles (3) comprend en outre au moins un élément choisi parmi le groupe comprenant le Pt et le Pd en tant que l'ingrédient catalytique dans une quantité de charge allant de 0,5 à 2,0 g et de 0,5 à 2,0 g, respectivement, par rapport à volume apparent de 1 litre de chacun des supports en nid-d'abeilles (3, 4).
  10. Catalyseur de purification des gaz d'échappement (1) selon la revendication 7, dans lequel la couche catalytique disposée sur la surface du support en nid-d'abeilles (3, 4) à l'exception du premier support en nid-d'abeilles (3) comprend du Rh en tant que l'ingrédient catalytique selon dans une quantité de charge allant de 0,2 à 0,5 g par rapport à volume apparent de 1 litre du premier catalyseur.
  11. Catalyseur de purification des gaz d'échappement selon la revendication 10, dans lequel la couche catalytique disposée sur la surface des supports en nid-d'abeilles (3, 4) à l'exception du premier support en nid-d'abeilles (3) comprend en outre au moins un élément choisi parmi le groupe comprenant le Pt et le Pd comme ingrédient catalytique dans une quantité de charge allant de 0,5 à 2,0 g et de 0,5 à 2,0 g, respectivement, par rapport à volume apparent de 1 litre de chacun des supports en nid-d'abeilles (3, 4).
EP04293173A 2004-01-29 2004-12-30 Catalyseur pour la purification des gaz d'échappement Expired - Lifetime EP1561509B1 (fr)

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JP2004021873A JP4503304B2 (ja) 2004-01-29 2004-01-29 排ガス浄化用触媒

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TWI316422B (en) 2009-11-01
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US7585478B2 (en) 2009-09-08
US20050170953A1 (en) 2005-08-04
EP1561509A1 (fr) 2005-08-10
JP2005211794A (ja) 2005-08-11
CN1669647A (zh) 2005-09-21
TW200528187A (en) 2005-09-01
CN100540138C (zh) 2009-09-16

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